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一种固定在二氧化硅包覆磁性纳米颗粒上的锰(III)席夫碱配合物,对硫化物和烯烃氧化表现出增强的电化学催化性能。

A manganese(iii) Schiff base complex immobilized on silica-coated magnetic nanoparticles showing enhanced electrochemical catalytic performance toward sulfide and alkene oxidation.

作者信息

Rayati Saeed, Khodaei Elham, Nafarieh Parinaz, Jafarian Majid, Elmi Bahareh, Wojtczak Andrzej

机构信息

Department of Chemistry, K. N. Toosi University of Technology P. O. Box 16315-1618 Tehran 15418 Iran

Faculty of Chemistry, N. Copernicus University Gagarina 7 87-100 Torun Poland.

出版信息

RSC Adv. 2020 Apr 30;10(29):17026-17036. doi: 10.1039/d0ra02728f. eCollection 2020 Apr 29.

DOI:10.1039/d0ra02728f
PMID:35496932
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9053262/
Abstract

In this study, a novel Mn(iii)-Schiff base complex was synthesized and characterized. The structure of this complex was determined to be a deformed octahedral coordination sphere by single-crystal X-ray diffraction analysis. The Mn(iii)-Schiff base complex was supported on silica-coated iron magnetic nanoparticles axial coordination by one-step complex anchoring to produce a heterogenized nanocatalyst. After this, the complex was characterized by Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDX), thermogravimetric analysis (TGA), vibrating sample magnetometry (VSM), and powder X-ray diffraction (XRD). Moreover, atomic absorption spectroscopy was used to determine the amount of the loaded metal. The heterogenized nanocatalyst effectively catalyzed the oxidation of a broad range of sulfides and alkenes with HO in the presence of a glassy carbon electrode, applying voltage to the reaction mixture. The results showed that the application of a potential to the reaction mixture could significantly decrease the reaction time when compared with the case of similar chemical oxidation reactions. In addition, an excellent value of turnover frequency (17 750 h) was achieved for the electrochemical oxidation of styrene. Moreover, the nanocatalyst showed good recoverability without significant loss of its activity within six successive runs in the electrochemical oxidation of methyl phenyl sulfide and cyclooctene. The electrochemical properties and stability of FeO@SiO-[MnL(OAc)] were investigated by cyclic voltammetry measurements and chronoamperometry technique.

摘要

在本研究中,合成并表征了一种新型的锰(III)-席夫碱配合物。通过单晶X射线衍射分析确定该配合物的结构为变形八面体配位球。通过一步络合锚定将锰(III)-席夫碱配合物负载在二氧化硅包覆的铁磁性纳米颗粒上进行轴向配位,以制备多相化纳米催化剂。此后,通过傅里叶变换红外光谱(FTIR)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)、能量色散X射线光谱(EDX)、热重分析(TGA)、振动样品磁强计(VSM)和粉末X射线衍射(XRD)对该配合物进行了表征。此外,使用原子吸收光谱法测定负载金属的量。在玻碳电极存在下,向反应混合物施加电压,该多相化纳米催化剂有效地催化了多种硫化物和烯烃与HO的氧化反应。结果表明,与类似化学氧化反应的情况相比,向反应混合物施加电势可显著缩短反应时间。此外,苯乙烯的电化学氧化实现了优异的周转频率值(17750 h)。此外,在甲基苯硫醚和环辛烯的电化学氧化反应中,该纳米催化剂在连续六次运行中显示出良好的可回收性,且其活性没有明显损失。通过循环伏安法测量和计时电流法技术研究了FeO@SiO-[MnL(OAc)]的电化学性质和稳定性。

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